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Use of the QIAGEN GeneReader NGS system for detection of KRAS mutations, validated by the QIAGEN Therascreen PCR kit and alternative NGS platform

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The detection of somatic mutations in primary tumors is critical for the understanding of cancer evolution and targeting therapy. Multiple technologies have been developed to enable the detection of such mutations.

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R E S E A R C H A R T I C L E Open Access

Use of the QIAGEN GeneReader NGS

system for detection of KRAS mutations,

kit and alternative NGS platform

Agus Darwanto1,7 , Anne-Mette Hein2, Sascha Strauss3, Yi Kong4, Andrew Sheridan1, Dan Richards4, Eric Lader5, Monika Ngowe1,8, Timothy Pelletier1, Danielle Adams1,9, Austin Ricker1, Nishit Patel1, Andreas Kühne3,

Simon Hughes6, Dan Shiffman4, Dirk Zimmermann3, Kai te Kaat3and Thomas Rothmann3*

Abstract

Background: The detection of somatic mutations in primary tumors is critical for the understanding of cancer evolution and targeting therapy Multiple technologies have been developed to enable the detection of such mutations Next generation sequencing (NGS) is a new platform that is gradually becoming the technology of choice for genotyping cancer samples, owing to its ability to simultaneously interrogate many genomic loci at massively high efficiency and increasingly lower cost However, multiple barriers still exist for its broader adoption

in clinical research practice, such as fragmented workflow and complex bioinformatics analysis and interpretation Methods: We performed validation of the QIAGEN GeneReader NGS System using the QIAact Actionable Insights Tumor Panel, focusing on clinically meaningful mutations by using DNA extracted from formalin-fixed paraffin-embedded (FFPE) colorectal tissue with known KRAS mutations The performance of the GeneReader was evaluated and compared to data generated from alternative technologies (PCR and pyrosequencing) as well as an alternative NGS platform The results were further confirmed with Sanger sequencing

Results: The data generated from the GeneReader achieved 100% concordance with reference technologies

Furthermore, the GeneReader workflow provides a truly integrated workflow, eliminating artifacts resulting from

routine sample preparation; and providing up-to-date interpretation of test results

Conclusion: The GeneReader NGS system offers an effective and efficient method to identify somatic (KRAS) cancer mutations

Keywords: GeneReader, Kras, Mutation, Cancer, Ngs

Background

Somatic mutations in the KRAS oncogene are common in

human cancers They are found in 70-90% of pancreatic

cancers [1, 2], 30-50% of colorectal cancers [3–5] and

Several methods have been developed for the detection of

KRAS mutations, each with specific advantages and

limitations [5, 9, 10]

Sanger sequencing has been the ‘gold standard’ for mutation analysis in cancer detection since the 1970s [11] However, limited by its low sensitivity (10-20% mutant allele frequency (MAF)) and low throughput [10], Sanger sequencing is no longer sufficient for the needs of today’s cancer molecular diagnostics

qPCR-based assay used to detect the most common KRAS mutations including those in codons 12 and 13 It has greatly improved sensitivity over Sanger sequencing, and has been approved by the Food and Drug Administration (FDA) [9] for colorectal cancer patient stratification

* Correspondence: Thomas.rothmann@qiagen.com

3 QIAGEN GmbH, QIAGEN Strasse 1, 40724 Hilden, Nordrhein-Westfalen,

Germany

Full list of author information is available at the end of the article

© The Author(s) 2017 Open Access This article is distributed under the terms of the Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made The Creative Commons Public Domain Dedication waiver

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Pyrosequencing also offers an attractive alternative to

Sanger due to its fast turnaround time (TAT) and lower

sensitivity threshold, even in tissues with low tumor cell

content [5]

Next-generation sequencing (NGS) differs radically

from the above mentioned methods Coupled with

amplicon-based targeting technology, NGS has the

cap-ability to simultaneously sequence in a massively parallel

way multiple genetic loci with minimal amounts of

nu-cleic acid input and limited time and expense [12–15]

This technology has revolutionized the speed of genetic

and genomic discovery, and advanced our understanding

of molecular mechanisms of diseases In recent years,

NGS has played an important role in advancing

person-alized healthcare and precision medicine by enabling the

identification of mutations associated with therapeutic

response or resistance As more clinically significant

genetic biomarkers and targeted therapies become

avai-lable, the profiling of such genetic variations is becoming

increasingly more critical Several NGS platforms are

already commercially available for sequencing and

iden-tification of genetic alterations associated with diseases,

such as point mutations, deletions, insertions and copy

number variants [16] However, QIAGEN’s GeneReader

System presented here includes all upstream sample

processing steps starting from nucleic acid extraction,

together with an integrated downstream bioinformatics

solution that enables a direct access to real-time updates

from the rapidly evolving literature, and clinical knowledge

and evidence

To this end, we recently evaluated the QIAGEN

GeneReader System workflow from DNA extraction and

purification from FFPE tissue samples, to library

prepa-ration, sequencing and data analysis and interpretation

Herein we show that the GeneReader presents a unified

workflow that provides accurate results and a simple

solution for any laboratory to use in clinical research

Methods

Sample and DNA isolation

FFPE Tumor material from colorectal cancer tumors

(Origene Technologies, MD, USA and Asterand

Biosci-ences, MI, USA) was used to prepare 56 DNA samples

with known KRAS mutation status, previously determined

using therascreen assay (Pyrosequencing and PCR) and

Sanger sequencing according to methods further described

below Tissue sections of 10μm in thickness, ranging from

3 to 20 years of age were used for DNA extraction utilizing

either: i) the QIAamp DNA FFPE Tissue Kit (QIAGEN,

Hilden, Germany) or ii) the GeneRead FFPE DNA Kit

(QIAGEN, Hilden, Germany) according to manufacturer’s

instructions DNA concentration was determined using

the Nanodrop System (Thermo Fisher Scientific, MA,

USA) and Qubit dsDNA HS assay (Life Technologies,

Gaithersburg, USA) The DNA was assessed using the GeneRead DNA QuantiMIZE System (QIAGEN, Hilden, Germany) which utilizes a qPCR-based approach to deter-mine the quality of sample DNA prior to NGS Further-more, both NA12878 (Coriell Institute for Medical Research) (for which the Genome in the Bottle (GIAB) consortium has published a set of high confident vari-ants [17]) and AcroMetrix (Thermo Fisher Scientific,

MA, USA) samples were used as a gold standard set of variant calls

GeneReader sample preparation and sequencing run

In total, 40 ng of DNA measured by Qubit (Thermo Fisher Scientific, MA, USA) was used as template to generate libraries for sequencing Libraries were pre-pared using the QIAGEN Library Kit v2.0 and the GeneRead QIAact Actionable Insight Tumor Panel (QIAGEN, Hilden, Germany), which amplifies 330 amplicons covering 16.7 kb, containing 773 unique variant positions in 12 genes (KRAS, NRAS, KIT, BRAF, PDGFRA, ALK, EGFR, ERBB2, PIK3CA, ERBB3, ESR1 and RAF1) All steps of library preparation were per-formed according to the manufacturer’s protocol The libraries were then quantified using a Qubit dsDNA HS Assay Kit (Life Technologies, MA, USA) and QIAxcel (QIAGEN, Hilden, Germany) Ten individual libraries were pooled prior to emulsion PCR and bead enrich-ment steps that were carried out using an automated protocol on the GeneRead QIAcube (QIAGEN, Hilden, Germany) using the GeneRead Clonal Amp Q Kit (QIAGEN, Hilden, Germany), according to the manu-facturer’s protocol Following bead enrichment, the pooled libraries were sequenced using the GeneReader platform (QIAGEN, Hilden, Germany)

GeneReader data processing

(QIAGEN, Hilden, Germany) was used to QC, align the read data to the hg19 reference genome sequence, call sequence variants, and generate an interactive report for visualization of the sequencing results, as well as a summary of the data QCI Analyze software reports a set of high- and low-confidence variants based on the coverage of variant positions Users have an option to analytically confirm if a variant listed should be valid or invalid before uploading to QCI Interpret software for the clinical interpretation For each sample the report was used to assess the quality of the overall sequencing run and to identify/call the individual variants After review, variants confirmed as analytically valid were uploaded to QCI Interpret for creation of a report for each sample based on detected variants and curated content, with a summary of findings and direct links to evidence sources

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Illumina MiSeq

The Actionable Insight Tumor Panel (QIAGEN, Hilden,

Germany) was used for a MiSeq (Illumina, CA, USA)

sequencing run The Kapa “with bead” PCR free protocol

(KAPABiosystems, MA, USA) was used in further Illumina

library preparation steps Samples were then paired-end

sequenced on a MiSeq instrument (Illumina, CA, USA)

according to Illumina guidelines The resulting reads were

mapped to the hg19 reference genome sequence using

BWA mem software followed by GATK (best practices) to

recalibrate base quality scores Variants were called using

MuTect Variants were then filtered using GATK (best

practice) and annotated using SnpEff Variants at hotspot

positions were selected using GATK

Pyrosequencing and Sanger analyses

The sample DNA obtained with the QIAamp FFPE

DNA Kit (QIAGEN, Hilden, Germany) was subjected to

Pyrosequencing analysis and Sanger sequencing For

Pyrosequencing the samples were analyzed using the

therascreen RAS Extension Pyro Kit (QIAGEN, Hilden,

Germany) which covers mutations in KRAS codons 59,

61, 117 and 146 as well as NRAS codons 59, 117 and

146 Samples with mutations in KRAS or NRAS codons

12 and 13 were further analyzed with the therascreen

KRAS or NRAS Pyro Kit (QIAGEN, Hilden, Germany)

according to manufacturer’s instructions In addition,

samples that failed the initial PyroMark KRAS analysis

were subjected to a second round of analysis Samples

with an initial“check” status, or with an indicated

muta-tion signal of LOD + 3% (“Potential low level mutamuta-tion”)

were subjected to a second round of analysis performed

in duplicate Sanger sequencing was performed using

Big Dye Terminator Technology and an ABI 3730xl

sequencer (Thermo Fisher Scientific, MA, USA)

Muta-tions were detected by analyzing the sequence trace files

and the quantity of a base at a certain position was

calculated from the area under the curve (AUC) at the

mutation specific position in the electropherogram

Therascreen qPCR

UK) is an allele-specific PCR-based technology with

spe-cific primers for the seven most common KRAS codon

12 and 13 mutations The assay screens for the following

mutations: 12 GCT (Ala), 12 GAT (Asp), 12 CGT (Arg),

12 TGT (Cys), 12 AGT (Ser), 12 GTT (Val), and 13

GAC (Asp) Mutation analysis was performed according

to manufacturer’s instructions, using the RotorGene

real-time PCR instrument (QIAGEN, Hilden, UK)

Ana-lysis of results was performed following the

recommen-dations in the manual, e.g samples with a control assay

with a cycle threshold (Ct) of 35 or higher were deemed

invalid and excluded from the analysis Samples were

called mutation positive based on the delta Ct values reported in the handbook Values over 40 cycles were scored as negative (wild-type)

Results

Evaluation of DNA quality by QuantiMIZE

FFPE samples with ages ranging from 3 to 20 years were used for this study The quality of the extracted DNA was measured by the GeneRead DNA QuantiMIZE QC assay (QIAGEN, Hilden, UK) Thirteen out of 56 samples failed quality checks and were excluded from further analysis (Additional file 1: Table S1) For the remaining 43 sam-ples, 3 to 9 PCR cycles were added (depending on the QuantiMIZE quality scores) to compensate for differences

in DNA quality during enrichment PCR The additional cycles ensured that poor quality (highly fragmented) DNA samples yielded enough material for downstream library preparation The quality of DNA purified from formalin fixated tissue decreases over the sample storage period time [18–20], but also depends on how tissues were treated, handled and processed before and during sample fixation [19, 21, 22]

GeneReader sequencing performance

The QIAact Actionable Insights Tumor Panel (QIAGEN, Hilden, UK) contains 773 unique variant positions in 12 genes (Table 1) An analysis of the reads mapped to the reference showed coverage levels that met the industry-standard 5% sensitivity criteria, even with aged FFPE samples A 200× minimum read coverage cutoff was used for calling a variant at any position in the panel For the 43 FFPE samples analyzed, an average amplicon coverage of 97.2% was observed, and an average variant insight coverage (hotspot coverage) of 99.8% was

samples, an average amplicon coverage of 98.5% was observed and an average variant insight coverage of 99.9% was observed at read depths of ≥200× (Table 1)

Table 1 Parameter and sequencing coverage of Actionable Insight Tumor Panel

Variant allele fraction detection limit 5%

Frequency cut-off and amplicon coverage >500×: 96.4% (A), 92.0% (B)

>200×: 98.5% (A), 97.2% (B) Frequency cut-off and variant insight

coverage

>500×: 99.8% (A), 98.6% (B)

>200×: 99.9% (A), 99.8% (B)

Positive samples included into the study have all been confirmed with Sanger sequencing and passed QuantiMIZE (<0.4) (A) An average of 12 NA12878 samples, (B) average of 43 colorectal cancers FFPE samples (ages 3-20 years)

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No false negatives (FN; where an expected variant was

not detected) were observed

Performance comparison between the QIAamp and

GeneRead DNA FFPE kits for DNA purification using the

GeneReader

Two DNA purification kits were used to isolate DNA from

FFPE samples Table 2 demonstrates the superior

perform-ance of the GeneRead DNA FFPE Kit (QIAGEN, Hilden,

UK) over the QIAamp DNA FFPE Tissue Kit (QIAGEN,

Hilden, UK) in terms of true positives at lower variant

call-ing sensitivity Fourteen true positive KRAS variants were

detected using an allele fraction cut-off of >5% for DNA

isolated by GeneRead DNA FFPE Kit (QIAGEN, Hilden,

UK) For the QIAamp DNA FFPE Tissue Kit (QIAGEN,

Hilden, UK), 15 KRAS variants were detected using an

allele fraction cut-off of >5% Of the 15 KRAS variants

detected, 14 were true positive variants and 1 was a false

positive (Table 2) as confirmed by several independent

methods Decreasing the allele fraction cutoff to >2.5%

re-sulted in identification of the same 14 KRAS true positive

samples for GeneRead DNA FFPE Kit (QIAGEN, Hilden,

UK) extractions However, for QIAamp DNA FFPE Tissue

Kit (QIAGEN, Hilden, UK) extracted samples at >2.5%

allele fraction cut-off, 11 additional false positive KRAS

mutations (25 variants in total) were detected The

additional mutations were mostly C to T transitions It is

known that FFPE fixation deaminates certain bases, most

prominently cytosine deamination to uracil [23–25] The

GeneRead DNA FFPE Kit (QIAGEN, Hilden, UK) contains

an integrated uracil DNA glycosylase (UDG) step which

removes uracil from the DNA before the final purification

step, yielding high-quality DNA with minimal artifacts

Confirmation of variants by MiSeq, pyrosequencing and

therascreen qPCR assays

The GeneReader NGS System variant calls demonstrated

100% agreement with KRAS mutation status previously

qPCR (Table 3) Of the 43 samples, 14 tested positive for

KRAS variants and 29 samples were confirmed as wild

type The 5% allelic fraction cut-off was used to call

KRAS variants for codons 12, 13, 59, 61, 117 and 146

The true positive variants observed by the GeneReader

NGS System share a 100% concordance with

MiSeq-Illumina (Table 4)

The use of the NA12878 control (Fig 1, Additional file 2: Table S2) and AcroMetrix (Fig 1, Additional file 3: Tables S3) reference standard materials

platform on high frequency and low frequency variants, respectively NA12878 has been used extensively as a ref-erence standard material for verifying NGS platforms [17] and acts as a useful control in establishing background error Besides its use as a GeneReader platform perform-ance standard, AcroMetrix has also been used previously

as a control for variant calls [26]

Discussion

A major advantage of NGS over traditional mutation detection methods is the ability to sequence multiple genes and variants simultaneously Other advantages include minimal DNA input, faster turnaround time;

Table 2 The GeneReader FFPE DNA sample preparation kit

successfully corrects FFPE artifacts

Type of DNA purification kit Allele frequency cut off

Table 3 KRAS agreement study between GeneReader and Pyrosequencing andTherascreen PCR Assays

>5% KRAS variant allele frequency cut off

Pyrosequencing and Therascreen PCR Assays (a)

(a)

If KRAS is mutant by Therascreen KRAS RGQ PCR assay or Therascreen RAS extension Pyrosequencing assay, the condition is recorded as a mutant (MT)

(b)

For Actionable Insights Tumor Panel, a 5% allelic frequency cut off was used

to call variants for codon 12, 13, 59, 61, 117 and 146, which are addressed by established QIAGEN Therascreen PCR assays

Table 4 The concordance study between GeneReader, MiSeq, PyrosequencingandTherascreen PCR assays

Sample no.

KRAS AA change

KRAS variant allele fraction (%) Therascreen PCR/Pyro GeneReadera MiSeqa

+: Variant identified by Therascreen PCR; allele fraction not available

a

: Sample processed from different FFPE section with potentially different

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lower overall cost and higher throughput and sensitivity

compared to traditional methods [12, 27–29] NGS has

revolutionized the speed of genetic and genomic

discov-ery, and advanced our understanding of the molecular

mechanisms of disease and potential treatment options

However, several major hurdles remain and still prevent

NGS from being broadly adopted in clinical practice

This is especially true for laboratories that are new to this technology, and may lack the in-house expertise required for processing complex bioinformatics data and interpretation of results Such expertise is crucial to construct a bioinformatics pipeline and to evaluate the software and generate quality reports The QIAGEN GeneReader NGS System allows users to perform

Fig 1 Variant calling performances of GeneReader pipeline Each individual data point was generated from 18 data points (a) NA12878 and (b) AcroMetrix Oncology Hotspot

Fig 2 QCI Analyze report showing the alignment of the reads at the variant positions along with the induced amino acid change

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experiments from sample to insight, tissue sample to

decipherable report based on the interpretation of

sequence variants detected

Analyze’ and ‘QCI Interpret’ for bioinformatics analysis and

reporting of variants, including read mapping, variant

call-ing and interpretation of results It provides visualization of

the alignment of sequencing results (Fig 2) as well as a

summary of the data Quality assessment is also supported,

both at the overall sequencing run level and for the analytic

validity of individual variants to reduce false positive and

negative results Using the data visualization tools within

QCI Analyze, it is possible to determine the quality of the

results and assess any variants of interest Further analysis

of variants using QCI Interpret provides access to the

curated information contained within the QIAGEN

Know-ledge Base enabling a deeper analysis and interpretation of

results for each sample (Fig 3) With all relevant

informa-tion, a report can be created with a summary of findings

and direct links to evidence sources At the single variant

level the QCI software is able to identify an individual

vari-ant as an actionable cancer mutation, and provides links to

current clinical research insights, e.g the KRAS G12D

somatic variant it is established to confer resistance to the

colorectal cancer drugs cetuximab and panitumumab,

based on evidence curated from their FDA drug labels and

clinical practice guidelines Within QCI-Interpret

informa-tion on active clinical trials recruiting colorectal cancer

patients with particular mutations are provided with drug,

nearest location, and trial phase information

The relationship between FFPE DNA quality and se-quencing accuracy is a critical point for any sese-quencing analysis The GeneReader workflow starts with the Gene-Read FFPE DNA Kit for DNA extraction and is specifically designed to reduce artifacts known to commonly occur in FFPE treated samples As seen in Table 2, by using FFPE samples aged from 3 to 20 years, the GeneRead FFPE DNA Kit successfully reduced the number of low quency false positive variants detected These low fre-quency false positive variants are likely caused by cytosine deamination and other fixation associated artifacts Similar phenomena were observed by Bourgon [23], where pre-treatment of FFPE samples with uracil DNA glycosylase (UDG) resulted in a dramatic reduction of false positives, with overall reductions of 77% for C > T and 94% for

G > A changes, respectively Biochemical removal of de-aminated DNA eliminates deamination-associated false positive results; however, for samples with very low quality DNA such as highly fragmented FFPE treated samples, UDG-treated may constitute an issue, as the treatment in-troduces possible further strand breaks leading to even higher fragmentation and lower availability of intact tem-plate strands Therefore, using the QuantiMIZE assay to identify those samples suitable for sequencing, based on

an assessment of original intact and amplifiable templates, before starting an experiment is a critical point for an amplification based NGS technology Previous reports ob-served that samples with lower amounts of amplifiable DNA are more likely to give a markedly increased number

of false positive results [30, 31]

Fig 3 QCI Interpret actionable report, showing summary of findings and link to the insights that can be used to guide clinical research

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In summary, this study confirms that the GeneReader

NGS System performs consistently and accurately in the

identification of somatic mutations from FFPE samples,

with results confirmed by both alternative technologies

as well as an alternative NGS platform With a full

end-to-end solution with integrated sample preparation and

bioinformatics interpretation, the GeneReader NGS

System is suitable for any laboratory interested in cancer

clinical research

Additional files

Additional file 1: Table S1 The QC results of the extracted DNA

samples were measured using GeneRead DNA QuantiMIZE (DOCX 28 kb)

Additional file 2: Table S2 List of NA12878 Gold Standard Variants

from 18 samples sequenced by GeneReader (DOCX 27 kb)

Additional file 3: Table S3 List of AcroMetrix ™ Oncology Hotspot

Gold Standard Variants from 18 samples sequenced by GeneReader

(DOCX 28 kb) (DOCX 27 kb)

Abbreviations

Ct: Cycle threshold; DNA: Deoxyribonucleic acid; dsDNA: Double-stranded

DNA; FDA: Food and Drug Administration; FFPE: Formalin-fixed

paraffin-embedded; GR: GeneReader; NGS: Next generation sequencing; NSCLC:

Non-small cell lung cancer; PCR: Polymerase chain reaction; qPCR: Quantitative

PCR; QC: Quality control; QCI: QIAGEN clinical insight; TAT: Turn-around time;

UDG: Uracil-DNA glycosylase

Acknowledgements

We greatly appreciate Drs Scott Steelman, Kathleen Steinmann and Robert

Lintner from Broad Technology Labs (Broad Institute of MIT and Harvard, 75

Ames Street (Rm 8021), Cambridge, MA 02141) for their support in samples

processing, GeneReader testing, and manuscript revisions We thanks to Drs.

Vikas Gupta, Naomi Thompson Kiran Divakar and Dietrich Lueerssen from

QIAGEN for the input of the manuscript.

Funding

This work was supported by QIAGEN.

Disclaimer

The sequencing chemistry used in this manuscript is currently available outside

the US The GeneReader NGS System is for research use only An upgraded and

different sequencing chemistry has meanwhile been made available in the US

since April 2017 and will become available worldwide later in 2017 For the

release of the new sequencing chemistry in the US in April, we have shown

equivalency to the sequencing chemistry used in the manuscript.

Availability of data and materials

The analyzed data sets generated during the study are available from the

corresponding author on reasonable request.

Authors ’ contributions

AD, AMH, SS, AS, EL, SH, TR designed the study AD, AMH, SS, AS, DR, MN, TP,

DA, AR, NP, DS, TR performed experiments and analyzed data AD, YK and TR

wrote the manuscript AK, DS, DZ, KK assisted in preparing the manuscript.

All authors read and approved the final manuscript.

Competing interests

At the time of the work was being done the authors where employees of

QIAGEN, and QIAGEN funded the research and the publication costs We

declare that our current or previous employment with QIAGEN did not

influence our interpretation of data or presentation of information.

Consent for publication

Ethics approval and consent to participate FFPE Tumor material from colorectal cancer tumors (Origene Technologies,

MD, USA and Asterand Biosciences, MI, USA) We refer to Origene ’s and Asterand ’s quality system as well as ethics and compliance processes with informed consent for commercial clinical samples We expect Origene and Asterand to follow industry standard ethics approval and consent processes.

Publisher’s Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Author details

1 QIAGEN Waltham, 35 Gatehouse Dr, Waltham, MA 02451, USA 2 QIAGEN Arhus, Silkeborgvej 2, 8000 Aarhus, Denmark 3 QIAGEN GmbH, QIAGEN Strasse 1, 40724 Hilden, Nordrhein-Westfalen, Germany 4 QIAGEN Redwood City, 1700 Seaport Blvd, Redwood, CA 94063, USA.5QIAGEN Frederick, 6951 Executive Way, Frederick, MD 21703, USA 6 QIAGEN Manchester, Skelton House Lloyd Street North, Manchester M15 6SH, UK 7 Novartis Institutes for BioMedical Research, Cambridge, MA 02139, USA 8 T2 Biosystems, Lexington,

MA 02421, USA.9Macherey-Nigel, Bethlehem, PA 18020, USA.

Received: 28 November 2016 Accepted: 5 May 2017

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